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Polycyclic Aromatic Hydrocarbons in Human Milk of Nonsmoking U.S. Women SUNG R. KIM,* ROLF U. HALDEN, AND TIMOTHY J. BUCKLEY† Department of Environmental Health Sciences Johns Hopkins Bloomberg School of Public Health, 615 N. Wolfe Street, Baltimore, Maryland 21205
Received September 10, 2007. Revised manuscript received November 23, 2007. Accepted January 8, 2008.
The determination of polycyclic aromatic hydrocarbons (PAHs) in human milk is relevant in assessing the dose to mothers and infants. Since measurements for the United States are lacking, we analyzed 13 PAHs in human milk from 12 nonsmoking American mothers. Analytes were extracted from milk by using a combination of centrifugation, liquid–liquid, andsolid-phaseextractiontechniques.Followingmethodvalidation with spiked bovine milk, PAH concentrations in human milk were determined by isotope dilution gas chromatography/mass spectrometry. Phenanthrene, fluorene, fluoranthene, and pyrene were found at median concentrations of 11.8, 3.0, 1.6, and 1.1 ng/g milk fat, respectively, whereas 9 additional analytes including benzo[a]pyrene were not detected ( pyrene. These rankings are consistent with those reported for urban ambient air (1, 2, 7). In contrast to the similarity observed with the Japanese study, PAH concentrations detected in milk from Italian nonsmokers were between 1.6 and 15.5 fold higher for phenanthrene and pyrene, respectively, than those obtained in the current study. In addition, the PAH rank order of phenanthrene > fluorene > pyrene > fluoranthene for human milk from Italy (14) was somewhat different from what we and others (15) have observed. From the data available, it is not clear if differences in concentration level and rank can be attributed to exposure (7, 40, 41) (i.e., indoor and outdoor air quality, secondhand smoke exposure status, or diet), the method of milk collection, or the method of analysis. The PAH concentrations observed in milk translate into median daily infant dose estimates for fluorene, phenan-
threne, fluoranthene, and pyrene of 18.8, 75.8, 9.1, and 6.1 ng/kg/day, respectively. To place the ingested PAH dose into context, we further estimated the likely magnitude of inhalation doses. Here, we relied on published indoor, outdoor, and personal PAH concentrations for U.S. cities, since measurements of airborne PAHs were not made as part of the current study. Using the air contamination values identified in the Supporting Information, we show that the relative contribution from inhalation and ingestion varies by PAH. For fluoranthene and pyrene, there is a near equal contribution from inhalation and ingestion with median doses of 9.9 vs 9.1 and 6.1 vs 6.1 ng/kg day, respectively. However, for fluorene and phenanthrene, with median ingestion doses of 18.8 and 75.8 ng/kg day vs inhaled doses of 4.3 and 34.5 ng/kg day, the ingested dose was clearly the dominant pathway of exposure, accounting for 81.4 and 68.7% of the combined dose from both sources. Since there are no health-based guidelines or standards for PAHs in human milk, we used the margin of exposure (MOE) (ratio of reference dose (RfD) to estimated dose) to assess the infant PAH hazard. The health hazard basis for the reference dose for fluorene is “decreased red blood cell, packed cell volume and hemoglobin”; for fluoranthene it is described as “nephropathy, increased liver weights, hematological alterations, and clinical effects”; and for pyrene it is characterized as “kidney effects including renal tubular pathology, decreased kidney weights” (42). There is no RfD for phenanthrene. The MOEs ranged from 2.1 × 10-3 (fluorene) to 4.9 × 10-3 (pyrene), indicating that the estimated milk ingestion doses for infants were more than 3 orders of magnitude lower than the threshold levels of known health concerns. However, it is important to note that the MOE related health effects were not evaluated for nursing infants. The initial measurements of PAH concentrations in human milk provided here for American nonsmoking women suggest that the average exposure of U.S. infants from breastfeeding is comparable to that reported for other parts of the world. Current dogma holds that the health benefits to the mother and the infant from nursing by far outweigh any risks from environmental chemicals found in milk. Findings of the current study support this position for PAHs, VOL. 42, NO. 7, 2008 / ENVIRONMENTAL SCIENCE & TECHNOLOGY
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FIGURE 2. Distribution of infant average daily dose (ng/kg day) by ingestion and inhalation. Each box shows the median as a center bar, 25th and 75th percentiles as a box, and 10th and 90th percentile values as whiskers.
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a group of ubiquitous environmental contaminants showing a propensity for partitioning into human milk.
Acknowledgments This study was supported through pilot funding from the Johns Hopkins NIEHS Center for Urban Environmental Health (ES 03819) and the U.S. EPA (R 827436), as well as the Johns Hopkins Center for a Livable Future. We thank Dr. Benjamin Blount for his sampling and analysis assistance and expertise, Dr. Penny Anderson for her assistance with human subject recruitment and sample collection, Dr. Judy LaKind for her valuable advice, and Ms. Karen Mancini at Maternity Center East for assisting with human subject recruitment.
Supporting Information Available Table of literature reports of median personal, indoor and outdoor PAH levels, and associated references. This material is available free of charge via the Internet at http:// pubs.acs.org.
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